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Physics Procedia 90 (2017) 305 – 312

Conference on the Application of Accelerators in Research and Industry, CAARI 2016,

30 October – 4 November 2016, Ft. Worth, TX, USA

Verification of plutonium content in PuBe sources using MCNP®

6.2.0 beta with TENDL 2012 libraries
M.L. Lockharta*, G.E. McMatha
a
Los Alamos National Laboratory, Los Alamos, NM 87545, USA

Abstract

Although the production of PuBe neutron sources has discontinued, hundreds of sources with unknown or inaccurately declared
plutonium content are in existence around the world. Institutions have undertaken the task of assaying these sources, measuring,
and calculating the isotopic composition, plutonium content, and neutron yield. The nominal plutonium content, based off the
neutron yield per gram of pure 239Pu, has shown to be highly inaccurate. New methods of measuring the plutonium content allow
a more accurate estimate of the true Pu content, but these measurements need verification. Using the TENDL 2012 nuclear data
libraries, MCNP6 has the capability to simulate the (α, n) interactions in a PuBe source. Theoretically, if the source is modeled
according to the plutonium content, isotopic composition, and other source characteristics, the calculated neutron yield in MCNP
can be compared to the experimental yield, offering an indication of the accuracy of the declared plutonium content. In this study,
three sets of PuBe sources from various backgrounds were modeled in MCNP6 1.2 Beta, according to the source specifications
dictated by the individuals who assayed the source. Verification of the source parameters with MCNP6 also serves as a means to
test the alpha transport capabilities of MCNP6 1.2 Beta with TENDL 2012 alpha transport libraries. Good agreement in the
comparison would indicate the accuracy of the source parameters in addition to demonstrating MCNP’s capabilities in simulating
(α, n) interactions.

© 2017 The
Published Authors.B.V.
by Elsevier Published by open
This is an Elsevier
accessB.V.
article under the CC BY-NC-ND license
Peer-review under responsibility of the Scientific Committee of the Conference on the Application of Accelerators in Research
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review
and Industry. under responsibility of the Scientific Committee of the Conference on the Application of Accelerators in Research and Industry

Keywords: MCNP, (α,n), PuBe, isotopic composition, neutron yield

* M.L. Lockhart. Tel.: +1-505-500-6963

E-mail address: mlockhart@lanl.gov

1875-3892 Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
Peer-review under responsibility of the Scientific Committee of the Conference on the Application of Accelerators in Research and Industry
doi:10.1016/j.phpro.2017.09.016
306 M.L. Lockhart and G.E. McMath / Physics Procedia 90 (2017) 305 – 312

1. Introduction

Over several decades, PuBe (Plutonium Beryllium) neutron sources have been produced worldwide. However,
production of these sources was discontinued in the 1980s due to nuclear safeguard and security issues posed by their
nuclear material content (Bagi et al. 2016). Although these sources are rarely in use today, hundreds still exist around
the world, including Russia and Hungary. The certificate and manufacturer information for these sources are often
very limited and in some cases only include the source type. When more information is provided, it can include the
calculated nominal plutonium content and the neutron yield measured at the time of manufacturing in addition to
source dimensions. In most cases, the manufacturers use the measured neutron yield and specific neutron yield per
gram of pure 239Pu when calculating the plutonium content (Bagi et al. 2004). This isotope of plutonium has a
comparatively lower yield than other isotopes, causing the nominal value of the Pu content to be significantly higher
than the actual Pu content, in some cases by a whole order of magnitude. The difference in the nominal and actual
plutonium content in these sources makes them difficult to identify and invites complications when reported to and
inspected by the International Atomic Energy Agency (IAEA) (Nguyen et al. 2006).
The neutron yield and the composition of the source will vary from the original because 241Pu beta decays into
241
Am, which produces a larger number of neutrons from (α, n) interactions. In addition, the neutron yields of different
isotopes of plutonium can vary by multiple orders of magnitude. For example, the specific yield for 238Pu is ~107 n/sg
while the yield for 241Pu is ~104 n/sg (Nguyen et al. 2006). The comparatively low yield of 241Pu accounts for the
significantly high calculated nominal plutonium content and the varying neutron yields show the importance of
knowing the isotopic composition of the plutonium in a source. Methods of determining the isotopic composition
include, but are not limited to, the use of the Multi-Group Analysis (MGA) algorithm to analyze the gamma spectra
(Nguyen et al. 2006) and High Resolution Gamma Spectrometry (HRGS) (Dryák et al. 2014). When determining the
plutonium content, isotopic composition, or neutron yield of a source, any two of the three can theoretically be used
to calculate the third.
Because the nominal value of plutonium content for many sources is highly inaccurate, institutions have undertaken
the task of measuring the neutron yield and isotopic composition of the source to determine the actual plutonium
content. The purpose of this study is to model the neutron sources described by studies published in previous papers
(Nguyen et al. 2006) (Anderson et al. 1972) (Dryák et al. 2014) in MCNP6® (Monte Carlo radiation-transport code).
Using both measured and calculated plutonium content, isotopic composition, and other specifications, a comparison
is made between the experimental and theoretical neutron yield. This comparison provides a benchmark and
verification of the source characteristics while also testing the TALYS Evaluated Neutron Data Library TENDL 2012
(Koning et al. 2012).
The TENDL libraries provide the outputs of the code TALYS (Koning et al. 2013), which was developed to
simulate nuclear reactions involving neutrons, photons, protons, deuterons, tritons, alphas and 3He particles, in the 1
KeV - 200 MeV energy range (Koning et al. 2013). Beginning in 2008, TENDL publicly released ACE (A Compact
Evaluated Nuclear Data File) formatted libraries. After the release of MCNP6® 1.1 beta, MCNP6 possessed the
capability to read the ACE libraries. Before this capability, MCNP6 used physics models instead of the ACE libraries
when simulating the transport of alpha particles (Pelowitz et al. 2014). Here, the models use the TENDL 2012 libraries
for alpha transport rather than TENDL 2014 due to pointers in the ACE files that are not usable in MCNP (Koning et
al. 2014).
Using the TENDL libraries, the ability of MCNP6 to model (α, n) interactions can be tested and benchmarked for
future modeling purposes. The sources presented here are small, but serve as an indication of the success of modeling
alpha transport in MCNP. This capability in MCNP6 will allow verification of source specifications in addition to
modeling other scenarios of interest to the Domestic Nuclear Detection Office (DNDO).

2. Method

When calculating the neutron yield of a source through a model, specific parameters must be known in order to
accurately represent the source and obtain the expected neutron yield. The most significant measurements include the
Be/Pu atomic ratio, the isotopic composition of plutonium, density, and the mass of plutonium (Bagi et al. 2016). The
Be/Pu ratio is often unspecified and is crucial in determining the mass of the Be based on the plutonium content. The
 M.L. Lockhart and G.E. McMath / Physics Procedia 90 (2017) 305 – 312 307

density is also important because it will affect the probability of a reaction occurring. The isotopic composition and
plutonium content will be given and these measurements need verification. MCNP requires an input deck in which the
model specifications are described and the physics options are specified. An example of an input deck is in the
Appendix. Specific lines of the deck are explained in the following paragraphs.
Most manufactured sources are cylindrical in shape. However, information concerning the thickness and size of the
container and uncertainty about the size of the nuclear material inside the container is limited and invites complications
and inaccuracy in a model. When verifying the neutron yield of a source through computer models, the shape will
have minimal effect on the yield, unless drastically different than the source in real life. Therefore, all sources were
modelled as a sphere with a radius calculated to ensure the correct density and mass as specified in the individual
source parameters. The source definition uses a particle type that is represented by a distribution of the activity of the
different isotopes within the source i.e. plutonium isotopes and beryllium. This distribution is even within a sphere of
a set radius and centered at the origin. The material card for each source includes all relevant isotopes of plutonium
and beryllium and the percentages are calculated and based on a 13/1 atomic ratio and the isotopic composition of
plutonium provided for each source.
Various physics options can be defined by the data cards in MCNP; some of the options relevant to this model are
described briefly below. The TENDL 12 libraries are used for the alpha transport in beryllium while the physics models
are used for plutonium and americium. Using the TENDL 12 libraries, the lowest energy cross section is at 1 MeV;
therefore, the CUT card is used to change the lower energy cutoff from the default of 4 MeV to 1 MeV. The third and
fourth entries on the CUT card are also set to zero, which invokes analog capture. The ACT card is used to turn off
creation of delayed particles from fission events (FISSION=none) and to create delayed alphas from non-fission events
(NONFISS=a). The HLCUT keyword is present on the ACT card and is set to 0.01 to truncate the decay chain after
the first decay (Pelowitz et al. 2014). An F1 surface tally is also present on the outside surface of the sphere to count
the neutrons emitted by the source.
Computer time for running charged particle simulations in MCNP6 is significant. Each input deck was run
using 1e9 histories to ensure a statistically accurate answer, resulting in approximately 1000 computer hours per
simulation. Running a large number of histories helps ensure a small relative error. It is also important that the tally
converges and passes all 10 statistical checks. Passing all 10 statistical checks is a good indication to the user that there
has been an adequate number of samples to conclude that the resulting value is accurate.

3. Results

The source IDs listed in all tables are consistent with the manufacturer assigned ID listed in the papers. Sources
NZ010 and NZ022 are of Russian provenience and are currently under the ownership of the Czech Metrology Institute-
Inspectorate for Ionizing Radiation (CMI-IIR) and are listed in a reference (Dryák et al. 2014). The next eight sources
listed in Tables 1 and 2, from 0.2-480 to 85-701, are Soviet manufactured and are currently in the possession of the
Institute of Isotopes at the Hungarian Academy of Sciences (Lakosi et al. 2006). Sources M-99, M-977, M-591, and
M-930 were all manufactured in Mound Laboratory in Miamisburg, Ohio, United States of America for experimental
purposes and are documented (Anderson et al. 1972).
For the Hungarian sources described by Nguyen and Dryák, based on conversion factors obtained both
experimentally and theoretically, the conclusion was drawn that source alloy was in a 13/1 ratio in sources investigated
which is in agreement with other descriptions (Bagi et al. 2016). The 13/1 ratio was used for calculating the mass
percentage of beryllium as 32-35%, depending on the source. This is consistent with the mass percentages calculated
in sources described by Anderson, for which both the mass of the plutonium and beryllium are given. The density of
the Hungarian sources is 3.7 g/cm3 as given by Nguyen and Dryák while the Anderson sources have a density of 3.9
g/cm3. Based on the total mass and density of the source, the radii of the spheres range from 0.12-2.5 cm. The isotopic
composition of all 14 sources was given and is listed in Table 1.
308 M.L. Lockhart and G.E. McMath / Physics Procedia 90 (2017) 305 – 312

Table 1. Isotopic Composition of PuBe Sources in Mass Percentage

238 239 240 241 242 241
Source ID Pu Pu Pu Pu Pu Am
NZ010 1.3 76.5 15.6 1.5 - 5.0
NZ022 4.3 65.9 26.3 0.8 - 2.7
0.2-480 1.0 83 14 0.71 1.19 2.2
2-479 1.0 79.9 17 0.73 1.38 2.27
1.9-611a 0.004 95.6 4.3 0.046 0.014 0.23
4.7-555 0.0035 96 4.15 0.05 0.012 0.22
4-407 0.001 95 4.73 0.04 0.015 0.23
37-425 1.06 77 19.7 0.7 1.6 2.8
178-461 1.3 76 20.0 0.8 1.9 2.9
85-701 0.0076 95 5.0 0.044 0.017 0.22
M-99* - 97.0 3.0 0.1 - -
M-977* - 92.0 7.0 0.7 - -
M-591* - 95.0 5.0 0.4 - -
M-930* - 92.0 7.0 0.7 - -
*approximation in ref (Anderson et al. 1972)

The plutonium content was provided by various institutions and was either obtained by measurements or
calculations. For the Anderson sources, the exact plutonium content is known because they manufactured the sources
themselves and gave the approximate measurements. Gamma spectrometry was used to calculate the plutonium
content of sources described Dryák and the plutonium content is calculated based on the 129 and 413 MeV peaks.
These values are in Table 2 along with the nominal content of the sources. The plutonium content in the Hungarian
sources listed by Nguyen is determined using gamma peaks of relatively high intensity at different energies. Multiple
values for the plutonium content are calculated from the count rate at different gamma peaks, but only the counts at
375 and 413 MeV, which agree, are considered and used for calculating the plutonium content that is reported. These
8 sources had been assayed in years prior to the measurements provided by Nguyen and the previously calculated
plutonium contents (Bagi et al. 2004) (Lakosi et al. 2006) were larger than the values that were documented more
recently by Nguyen. Formerly, these sources were characterized by high-resolution gamma-spectrometry (HRGS) for
the isotopic analysis and a “combined method” (CBM) algorithm was used to calculate the plutonium content. The
method of calculating plutonium content was refined from that used by Bagi to the algorithm used by Lakosi. As old
methods are refined, and new methods are produced, the plutonium content becomes more accurate and easier to
verify through MCNP simulation when the source characteristics are documented and readily available for modeling.
The nominal value and the actual plutonium contents calculated using different methods in different references are
listed in Table 2. The measured plutonium content gets smaller with time, as better methods and techniques are
developed. MCNP simulation proves that the smaller values are more accurate.
 M.L. Lockhart and G.E. McMath / Physics Procedia 90 (2017) 305 – 312 309

Table 2. Nominal and calculated plutonium content in grams

Source ID Nominal 2004* 2006** Current***

0.2-480 0.18 0.0323 0.0282 0.020
2-479 1.8 0.277 0.294 0.205
1.9-611a 1.9 - 1.57 0.84
4.7-555 4.7 3.45 3.51 3.0
4-407 4 - 4.01 2.55
37-425 36 5.74 5.03 4.0
178-461 177 24.6 19.3 19.5
85-701 85 75.3 55.9 49.2
NZ010 540 - - 78.0
NZ022 540 - - 25.5

*calculation of plutonium in ref (Bagi et al. 2004)

**updated calculation of plutonium in ref (Lakosi et al. 2006)
***Pu content used in MCNP model. (Nguyen et al. 2006) (Dryák et al. 014)

Table 3. Comparison of neutron yields

Source ID Measured (n/s) Calculated (n/s) % Difference

NZ010 8.19E+07 7.41E+07 -9.6%
NZ022 4.89E+07 4.75E+07 -2.8%
0.2-480 1.17E+04 1.19E+04 1.7%
2-479 1.17E+05 1.23E+05 5.1%
1.9-611a 1.32E+05 1.13E+05 -14.4%
4.7-555 3.34E+05 4.03E+05 20.7%
4-407 2.99E+05 3.43E+05 14.7%
37-425 2.47E+06 2.75E+06 11.3%
178-461 1.14E+07 1.54E+07 35.1%
85-701 5.72E+06 7.04E+06 8.5%
M-99 2.00E+05 2.41E+05 20.7%
M-977 1.60E+06 1.73E+06 8.3%
M-591 8.90E+06 9.94E+06 11.7%
M-930 1.80E+07 2.41E+07 34.2%

Using all information provided, the models provide a means of verifying the accuracy of source parameters to a
certain degree. A comparison between the measured neutron yield of the source and the neutron yield calculated in
MCNP6 was made and the measurements, MCNP calculations, and the relative differences are in Table 3. From the
results, the plutonium content and the isotopic compositions calculated and measured are within an acceptable
percentage of the real value. A few of the neutron yields were larger by a greater percentage, which can have multiple
causes. The plutonium content calculated could be higher than the actual content. However, the plutonium in the
Anderson sources described by Anderson et al. (1972) was not calculated but known exactly by the manufacturer. A
higher neutron yield can also be explained by an inaccurate isotopic composition. As discussed previously, the specific
yield for different isotopes of plutonium and 241Am can vary by multiple orders of magnitude. Any difference in the
310 M.L. Lockhart and G.E. McMath / Physics Procedia 90 (2017) 305 – 312

composition of the model compared to the composition of the source itself can have a large effect on the total neutron
yield. For the Anderson sources, the isotopic composition was approximate as noted by Anderson; this can explain
the larger differences in the neutron yields. All other yield comparisons are within an acceptable margin of error,
excluding source 4.7-555 and 178-461. When making the neutron yield comparisons, the experimental measurements
are assumed to be accurate. However, it should also be noted that the experimental measurements for the neutron yield
of a source can be affected by the efficiency and type of neutron detector. High yield measurements can also be
affected by detector deadtime. When source is measured, the yield is corrected to account for detector efficiency and
deadtime, but these corrections become less effective for high yield measurements. This can cause the experimental
measurements to be lower than expected. In the comparison between experimental and calculated yields, most of the
calculated results are higher than the experimental. This observation provides a logical reason to extend the acceptable
margin of error when the calculated yield is significantly larger than the experimental measurements. In general, if
the MCNP simulation produces a larger neutron yield than the experimental value, it can be inferred that the plutonium
content is likely less than what was measured.

4. Conclusion

As new methods of source characterization are being developed, it is important to verify the accuracy of the
calculations. In the case of PuBe sources, this verification is valuable regarding nuclear safeguards and security due
to the presence of nuclear material. Sources need to be evaluated because the nominal plutonium content is often very
inaccurate and larger than the actual amount contained in the source. For example, in source 178-461 (Nguyen et al.
2006) the manufacturer listed the nominal plutonium content as being 177 g. When the source was assayed using
gamma-spectrometry, the actual plutonium content was found to be only 19.5 g and the neutron yield comparison
suggests a possibly lower plutonium content. The difference in these values is very significant and brings into question
our ability to identify and keep track of these sources when the nominal and actual specifications are different. The
exaggerated and highly inaccurate plutonium content report causes these sources to be classified in a higher category
of nuclear material than is necessary. Sources in higher categories have stricter requirements regarding physical
protection and administration that are unnecessary and wasteful if the source only contains a small percentage of the
nominal plutonium content (Dryák et al. 2014). However, in characterizing these sources, time can change the
accuracy of measurements. The total nuclear material content should not significantly change, but the composition
will vary as different isotopes decay. A change in composition will also affect the neutron yield, often increasing due
to the presence of 241Am. With new technology and ways of measuring the change in isotopic composition, the
plutonium content can still be verified using the latest isotopic measurements and neutron yield.
With hundreds of sources still in existence, it is important to have substantial knowledge regarding the
content of those sources in order to effectively establish regulations and safeguards. It should be noted that the sources
presented here have less importance in the view of safeguards, but does indicate the ability to assay larger sources.
Although methods of characterizing these sources have not been perfected, a calculated and verified approximation
allows for better identification and categorization then any inaccurate nominal information. A rough estimate of the
plutonium content can be made based using the total neutron yield, the isotopic composition, and the specific neutron
yield for each isotope. This provides a significantly more accurate value than the nominal content; however, it is often
an overestimate.
Using the ACE formatted libraries rather than physic models, MCNP6 does possess the capability to model
alpha transport at lower energies with reasonable accuracy. This is valuable for both source verification and future
simulations involving neutron sources. Various assay methods provide the ability to characterize and identify neutron
sources that have been found, seized, or transported, legally or illegally. However, it is necessary to have a way to
verify the accuracy of the measured source parameters or to model scenarios pertaining to nuclear security. MCNP6
is useful in verifying source specifications through a neutron yield comparison. Unfortunately, the computation cost
can cause limitations in a user’s ability to simulate a source. Currently, simulations for alpha transport require
thousands of computer hours. To produce the neutron yield in a timely manner, a biasing of secondary particle
production from alpha transport is necessary. Currently, no biasing for the neutron production from alpha sources
exists; however, a biasing algorithm has been developed, but is currently being tested and is unavailable to users.
 M.L. Lockhart and G.E. McMath / Physics Procedia 90 (2017) 305 – 312 311

Acknowledgements

This work has been supported by the U.S. Department of Homeland Security and the Domestic Nuclear Detection
Office (DNDO). This support does not constitute an express or implied endorsement on the part of the Government.

Appendix

Example of MCNP input deck:

0.2-480
1 1 -3.7 -1 imp: n,a,# = 1
2 0 1 -2 imp: n,a,# = 1
3 0 2 imp: n,a,# = 0

1 so 0.124338951 $ sphere of PuBe

2 so 0.5

mode n a #
sdef par = d1 pos = 0 0 0 cel = 1 rad =d2 erg=0 wgt=7.77e8
si1 L 94238 94239 94240 94241 94242 95241
sp1 1.61E-01 4.84E-02 2.99E-02 6.90E-01 4.42E-05 7.09E-02
si2 0 0.124338951
sp2 -21 2
ACT FISSION=none NONFISS=a HLCUT=0.001
f1:n 1
e1 1 94i 20
m1 94238 0.00492223 $ material specifications for PuBe, different for each source
94239 0.406836026
94240 0.068337075
94241 0.003451145
94242 0.005760418
95241 0.01069369
4009.12a 6.5
mx1:a MODEL 5r j
CUT:a j 1 0 0
CUT:n 2j 0 0
dbcn 9j 1e30
nps 1e9
print

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